CN109818021A - It is a kind of based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel cell - Google Patents
It is a kind of based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel cell Download PDFInfo
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- CN109818021A CN109818021A CN201811629494.4A CN201811629494A CN109818021A CN 109818021 A CN109818021 A CN 109818021A CN 201811629494 A CN201811629494 A CN 201811629494A CN 109818021 A CN109818021 A CN 109818021A
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- composite material
- ceo
- fuel cell
- solid oxide
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Abstract
The invention discloses a kind of based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel cell, and the cathode and anode of the fuel cell are the nickel foam that surface is coated with NCAL, and the electrolyte layer of the fuel cell is CeO2/Fe3O4Composite material.The structure of fuel cell i.e. of the present invention are as follows: nickel foam //NCAL//CeO2/Fe3O4//NCAL//nickel foam.Low-temperature solid oxide fuel cell of the present invention uses CeO2/Fe3O4Nanocomposite substantially reduces the electrode polarization loss during electrochemical reaction of fuel battery as its electrolyte layer；The electrolyte has high oxygen ion conduction ability in low-temperature zone, to make efficient stable to run for a long time using the solid oxide fuel cell of the electrolyte in low-temperature zone (300-600 degree).
Description
Technical field
The present invention relates to a kind of based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel cell,
Belong to field of new energy technologies.
Background technique
Chemical energy in fuel (such as hydrogen, methane) can be efficiently converted to electric energy by solid oxide fuel cell.
Transfer efficiency is not limited by Carnot cycle, and efficiency is much higher than thermal power generation unit.Fuel cell is electrolysed qualitative classification by it can
It is divided into Proton Exchange Membrane Fuel Cells, solid oxide fuel cell, alkaline fuel cell, molten carbonate fuel cell, phosphorus
Hydrochlorate fuel cell, wherein solid oxide fuel does not need that noble metal catalyst, material selection range be wide, high conversion efficiency
The advantages that, it receives significant attention.But current solid oxide fuel cell mainly uses yttria-stabilized zirconia
(YSZ) it is used as electrolyte, YSZ needs that higher catalytic activity could be obtained in high temperature (900 degree or so).Therefore traditional solid
Oxide fuel cell generally all operates in the condition of high temperature.Hot operation all proposes that harshness is wanted to battery material, connecting material
It asks, in addition, hot operation proposes challenge to solid oxide fuel cell long-time stability.Therefore research low-temperature zone (300-
600 degree) solid oxide fuel cell in recent years, cause extensive concern.
The widely used YSZ of the electrolyte of solid oxide fuel cell based on cathode-electrolyte-anode structure
(zirconium oxide of stabilized with yttrium oxide) completes the electrochemistry of fuel cell in 900 degree or so oxygen ion conduction abilities with higher
Reaction, electromotive power output.But the material (YSZ) only just has good oxygen ion transport ability at high temperature, works as temperature
600 degree are reduced to hereinafter, almost without oxygen ion conduction ability.Therefore, in recent years, about reduction solid oxide fuel cell
Technology it is more and more, be concentrated mainly on two technology paths, first is that develop thin film technique, be thinned electrolyte YSZ thickness, make
Its middle-temperature section also can ion transport capability with higher, but due to technical limitations, thickness can not infinitely subtract
It is thin, and thin film technique yield rate is also not very high；Second is that developing new material, the green wood of ion can be transmitted in low-temperature zone by finding
Material.
Fuel cell is a typical electrochemical device, and the effect of intermediate electrolyte is transmission ion and prevention electronics
Transmission.The doped semiconductor in ion conductor, it is easy to allow people to associate the generation of short circuit phenomenon, just because of this, have half
The material of conductor nature is so far without using in a fuel cell.The a large amount of experimental study of the present invention shows in ion conductor material
The material of semiconductor property, the especially semiconductor with perovskite structure or perovskite-like structure are suitably doped in material
Any short circuit phenomenon does not occur, but produces enhancement effect for material, and output power obviously increases.
Summary of the invention
Technical problem to be solved by the invention is to provide a kind of based on cerium oxide/ferriferrous oxide composite material low temperature
Solid oxide fuel cell, the electrolyte in the fuel cell are answering for nanoparticle material and nano semiconductor material
It closes, is formed with semiconductor-ion heterojunction structure in compound electrolyte material, the semiconductor-ion heterojunction structure may advantageously facilitate
The transmission speed of ion makes compound electrolyte material of the present invention have high conducting power to oxonium ion in low-temperature zone, to make
Using the electrolyte solid oxide fuel cell can efficient operation at low-temperature zone (300-600 degree).
In order to solve the above technical problems, the technical scheme adopted by the invention is as follows:
It is a kind of based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel cell, the fuel cell
Cathode and anode be that surface is coated with the nickel foam of NCAL, the electrolyte layer of the fuel cell is CeO2/Fe3O4Composite material.
The structure of fuel cell of the present invention are as follows: nickel foam //NCAL//CeO2/Fe3O4//NCAL//nickel foam.
Wherein, the nickel foam that surface is coated with NCAL is prepared with the following method: by the desired amount of NCAL
(Ni0.8Co0.15Al0.05LiO2-δ) powder is gradually added into terpinol, until mixture is starchiness, by starchy mixture
It is uniformly applied in nickel foam, the nickel foam after smearing is put into baking oven drying 2 hours at 200 DEG C, surface can be obtained
It is coated with the nickel foam of NCAL.
Wherein, the CeO2/Fe3O4Composite material is by CeO2With Fe3O4Using wet chemical one-step synthesis, by clear
It washes, filter, drying, being sintered, being fully ground acquisition.
Above-mentioned CeO2/Fe3O4The preparation method of composite material, specifically: by CeO2With Fe3O4In mass ratio 3: 1 mixing, obtain
To 4g mixed powder, mixed powder is put into 20mL deionized water, constant temperature stirs 4 hours, concentrated nitric acid is slowly added dropwise, until
Fe3O4Powder completely disappears, then suitable sodium carbonate liquor is added dropwise, and sufficiently after reaction, cleaning is filtered 4 times, be then dried,
Sintering processes are fully ground after sintering, obtain CeO2/Fe3O4Powder.
Wherein, the concentration of the sodium carbonate liquor is 0.5mol/L.
Wherein, be sintered with the heating rate of 10 DEG C/min, rise to 700 degree from drying temperature, be sintered 4 hours, then from
So it is cooled to room temperature.
Wherein, drying temperature is 120 degree, and drying time is 12 hours.
Material prepared by the present invention is composite nano materials, i.e., nanoparticle material and nano semiconductor material is compound,
Using grinding, form the nano combined of ionic material and semiconductor material, formed in this two-phase composite material semiconductor-from
Sub- heterojunction structure forms the interface of nanoelectronic phase with nanoparticle phase, nanoelectronic phase and nanometer in electrolyte layer
The interface of ion phase can reinforcement material to the transmittability of oxonium ion so that the output power of fuel cell dramatically increases；This
Outside, the mutual conversion between the iron of divalent and the iron of trivalent, also can be further improved the catalytic activity of composite material.
The preparation of low-temperature solid oxide fuel cell of the present invention:
The nickel foam that surface is coated with NCAL is fabricated to electrode, electrode size is circle, and diameter D=13mm, electrode is being received
Nano composite material CeO2/Fe3O4Both sides are in symmetrical structure, i.e. nickel foam //NCAL//CeO2/Fe3O4//NCAL//nickel foam knot
Piece of foam nickel //NCAL is put into compression mold bottom by structure, and surface is coated with the one side of NCAL upward, takes the CeO of 0.35g2/
Fe3O4Composite material is put into compression mold, then another nickel foam //NCAL is put into compression mold, is placed on CeO2/Fe3O4It is multiple
Above condensation material, surface be coated with NCAL one down, compression mold is put into tablet press machine, is forced into 8Mpa, after pressure maintaining 5 seconds,
Cell piece is taken out, low-temperature solid oxide fuel cell of the invention is obtained.
Compared with the prior art, technical solution of the present invention has the beneficial effect that
Low-temperature solid oxide fuel cell of the present invention prepares CeO using wet chemical one-step synthesis2/Fe3O4Composite wood
Material, obtains compound electrolyte material CeO of the invention after being fully ground2/Fe3O4, composite material can be improved the transmission of oxonium ion
Speed, therefore composite material has good output power in low-temperature zone, while compound electrolyte material can also reduce fuel electricity
Electrode polarization loss in the electrochemical reaction process of pond；Therefore make to exist using the solid oxide fuel cell of the electrolyte
Low-temperature zone (300-600 degree) being capable of long-term efficient stable operation.
Detailed description of the invention
Fig. 1 is the structural schematic diagram of low-temperature solid oxide fuel cell of the present invention；
Fig. 2 is two kinds of CeO2/Fe3O4Synthetic composite material and pure CeO2The fuel cell of electrolyte is being tested respectively
I-V and I-P characteristic curve when temperature is 550 degree；Under 550 degree of service condition, work as CeO2/Fe3O4Preparation process uses
NaCO3When precipitating, peak power output reaches 530mW/cm2；
Fig. 3 is CeO2/Fe3O4Synthetic composite material uses NaCO3Exchange when depositing technology under hydrogen-oxygen atmosphere
Impedance characteristic；
Fig. 4 is CeO2/Fe3O4Synthetic composite material is without NaCO3Exchange resistance when depositing technology under hydrogen-oxygen atmosphere
Anti- characteristic curve；
Fig. 5 is pure CeO2Ac impedance characteristic curve under hydrogen-oxygen atmosphere；
Fig. 6 is CeO2/Fe3O4The XRD diagram of composite material.
Specific embodiment
According to following embodiments, the present invention may be better understood.However, as it will be easily appreciated by one skilled in the art that real
It applies content described in example and is merely to illustrate the present invention, without sheet described in detail in claims should will not be limited
Invention.
As shown in Figure 1, the nickel foam that surface is coated with NCAL constitutes symmetry electrode, fuel battery negative pole of the present invention and anode are equal
The nickel foam of NCAL is coated with using surface, core electrolyte layer is CeO2/Fe3O4Composite material, therefore the structure of the fuel cell
Are as follows: nickel foam //NCAL//CeO2/Fe3O4//NCAL//nickel foam；Wherein, NCAL is the nickel cobalt aluminium lithium-of purchase
Ni0.8Co0.15Al0.05LiO2-δMaterial, CeO2/Fe3O4The composite material of Moist chemical synthesis preparation is utilized for the present invention；Nickel foam is quotient
The nickel material of the foam-like of industry purchase.
The preparation method of fuel cell of the present invention:
First prepare the nickel foam (anode and cathode as fuel cell) that surface is coated with NCAL: by NCAL
(Ni0.8Co0.15Al0.05LiO2-δ) powder is gradually added into terpinol, until mixture is starchiness, by starchy mixture
It is uniformly applied in nickel foam, the nickel foam after smearing is put into baking oven drying 2 hours at 200 DEG C, surface can be obtained
It is coated with the nickel foam of NCAL；
CeO is prepared again2/Fe3O4Composite material (electrolyte layer-generating element as fuel cell):
By CeO2With Fe3O4In mass ratio 3: 1 mixing, obtain 4g mixed powder, mixed powder are put into 20mL deionized water
In (CeO at this time2It is dissolved in the water, Fe3O4Do not dissolve in water), constant temperature stirs 4 hours, concentrated nitric acid is slowly added dropwise, until Fe3O4
Powder completely disappears (i.e. Fe3O4Powder is completely dissolved), then suitable sodium carbonate liquor (concentration 0.5mol/L) is added dropwise, when anti-
It answers after no longer generating new precipitating in liquid, stops that sodium carbonate liquor is added dropwise；Reaction solution is cleaned repeatedly, is filtered 4 times, will
To suction filtration object dried 12 hours in 120 degree of drying box, place into muffle furnace and be sintered 4 hours under 700 °, it is naturally cold
But to room temperature, after being fully ground, CeO is obtained2/Fe3O4Composite material, CeO2/Fe3O4In composite material, CeO2In in addition to doping
Outside the ferro element of each valence state, also doped with micro sodium ion.
Finally, combining electrode material obtained with electrolyte, low-temperature solid oxide fuel of the invention is obtained
Battery:
The nickel foam that surface is coated with NCAL is fabricated to electrode, electrode size is circle, and diameter D=13mm, electrode is being received
Nano composite material CeO2/Fe3O4Both sides are in symmetrical structure, i.e. nickel foam //NCAL//CeO2/Fe3O4//NCAL//nickel foam knot
Piece of foam nickel //NCAL is first put into compression mold bottom by structure, and surface is coated with the one side of NCAL upward, then takes 0.35g's
CeO2/Fe3O4Composite material is put into compression mold, and another nickel foam //NCAL is finally put into compression mold, is placed on
CeO2/Fe3O4Above composite material, surface be coated with NCAL one down, compression mold is put into tablet press machine, is forced into 8Mpa,
After pressure maintaining 5 seconds, cell piece is taken out, low-temperature solid oxide fuel cell of the invention is obtained.
Fig. 2 can be seen that experimental study shows pure CeO2Can also be used as the electrolyte of fuel cell, but output performance compared with
Difference, under 550 degree of test temperature, peak power output is only 72mW/cm2, and it is unstable；It is closed using one step of wet chemical
At CeO2/Fe3O4Composite material, by Fe3O4With CeO2It carries out compound, prepares nanocomposite, i.e. CeO2/Fe3O4Composite wood
Material, electrochemistry output performance is from 72mW/cm2Rise to 157mW/cm2, when NaCO is added dropwise in one-step synthesis technical process3Solution,
Output performance is obviously improved, and reaches 259mW/cm2。
In Fig. 3, CeO2/Fe3O4NaCO is used in composite material synthesis process3When depositing technology under hydrogen-oxygen atmosphere
Ac impedance characteristic curve and first intersection point of the imaginary axis represent ohmic loss, value is about 0.35 Ω cm2, AC impedance
Characteristic curve and second intersection point of the imaginary axis represent crystal boundary loss, and value is about 0.4 Ω cm2。
In Fig. 4, CeO2/Fe3O4Without NaCO in composite material synthesis process3When depositing technology under hydrogen-oxygen atmosphere
Ac impedance characteristic curve and first intersection point of the imaginary axis represent ohmic loss, and value is about 0.5 Ω cm2, AC impedance spy
Linearity curve and second intersection point of the imaginary axis represent crystal boundary loss, and value is about 1.8 Ω cm2。
In Fig. 5, pure CeO2Ac impedance characteristic curve and first intersection point of the imaginary axis represent ohmic loss, value is about
0.392cm2, second intersection point of ac impedance characteristic curve and the imaginary axis represent crystal boundary loss, and value is of about for 1.6 Ω cm2。
By comparison diagram 3, Fig. 4, Fig. 5 it is found that with pure CeO2Impedance operator compare, in synthesis process use NaCO3Precipitating
The CeO of technique preparation2/Fe3O4The ohmic loss of composite material and crystal boundary loss all substantially reduce, to prove answering after doping
The performance of condensation material, which has, greatly to be promoted.
Fe3O4It is a kind of oxide of complexity, wherein 1/3 is Fe2+, 2/3 be Fe3+, the present invention will by wet chemical
Fe3O4With CeO2Synthesis, and high temperature sintering prepare the composite material of nanostructure, using grinding, formed ionic material with
Semiconductor material it is nano combined, semiconductor-ion heterojunction structure is formed in this two-phase composite material, i.e., traditional ion leads
The electrolyte layer of body, which becomes one, has semiconductor-ion heterojunction structure electrolyte layer.With semiconductor-ion heterojunction structure
Electrolyte can reinforce the transmittability to oxonium ion, therefore electrolyte composite material is at low-temperature zone (300-600 °)
With good output power.
As shown in fig. 6, comparison blue CeO2Standard diagram, it can be seen that pure CeO2There is also in composite powder,
Secondly, there is a wave crest near 36 degree, and by being compared with the PDF card of standard, the wave crest and magnetic iron ore Fe+2Fe2+
The wave crest of 3O4 standard card is corresponding, therefore, by XRD diagram spectrum analysis it is found that Fe is entrained in CeO2In, and there is valence
State variation, the variation of Fe valence state strengthen the catalytic activity of composite material.This interpretation of result shows CeO2/Fe3O4Composite material
Chemical property improve mainly due to caused by the variation of Fe valence state, in XRD without discovery Na element, on the one hand may be
Since Na constituent content is very little, on the other hand the reduction of Na element may be led in suction filtration process.
The structure of fuel cell of the present invention, nickel foam are respectively used to anode and cathode to promote the redox reaction at the two poles of the earth
Process and play the role of electronics collection.The present invention is in pure CeO2It is middle to adulterate Fe using wet chemical3O4Material, in low-temperature zone
When operation, composite material has high oxygen ion conduction ability, to effectively increase the effect that fuel cell is run in low-temperature zone
Rate.
Claims (8)
1. a kind of based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel cell, it is characterised in that: institute
The electrolyte layer for stating fuel cell is CeO2/Fe3O4Composite material.
2. according to claim 1 based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel electricity
Pond, it is characterised in that: the cathode and anode of the fuel cell are the nickel foam that surface is coated with NCAL.
3. according to claim 2 based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel electricity
Pond, it is characterised in that: the nickel foam that surface is coated with NCAL is prepared with the following method: the desired amount of NCAL powder is added
Into terpinol, starchy mixture is obtained, starchy mixture is uniformly applied in nickel foam, can be obtained after drying
The nickel foam of NCAL is coated with to surface.
4. according to claim 1 based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel electricity
Pond, it is characterised in that: the CeO2/Fe3O4Composite material is to prepare CeO by one step of wet chemical2/Fe3O4Afterwards, it is fully ground
And it is made.
5. according to claim 4 based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel electricity
Pond, it is characterised in that: CeO2/Fe3O4The preparation method of composite material, specifically: by CeO2With Fe3O4In mass ratio 3: 1 mixing,
4g mixed powder is obtained, mixed powder is put into 20mL deionized water, constant temperature stirs 4 hours, concentrated nitric acid is slowly added dropwise, until
Fe3O4Powder completely disappears, then suitable sodium carbonate liquor is added dropwise, and sufficiently after reaction, cleaning is filtered 4 times, be then dried,
Sintering processes are fully ground after sintering, obtain CeO2/Fe3O4Composite material.
6. according to claim 5 based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel electricity
Pond, it is characterised in that: the concentration of the sodium carbonate liquor is 0.5mol/L.
7. according to claim 5 based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel electricity
Pond, it is characterised in that: sintering rises to 700 degree with the heating rate of 10 DEG C/min, from drying temperature, is sintered 4 hours, then from
So it is cooled to room temperature.
8. according to claim 5 based on cerium oxide/ferriferrous oxide composite material low-temperature solid oxide fuel electricity
Pond, it is characterised in that: drying temperature is 120 degree, and drying time is 12 hours.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111584911A (en) * | 2020-05-11 | 2020-08-25 | 合肥学院 | Fe3O4-BCFN intermediate temperature composite solid electrolyte and preparation method thereof |
| CN114068958A (en) * | 2021-11-16 | 2022-02-18 | 东南大学 | Method for preparing carbon nano tube by catalytic pyrolysis of waste plastics and applying carbon nano tube to low-temperature fuel cell |
| CN117410534A (en) * | 2023-11-08 | 2024-01-16 | 广东海洋大学 | Solid oxide fuel cell with symmetrical electrodes and preparation method thereof |
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| US20090011307A1 (en) * | 2007-07-04 | 2009-01-08 | Korea Institute Of Science And Technology | Electrode-Electrolyte Composite Powders For a Fuel Cell And Method For The Preparation Thereof |
| CN108808047A (en) * | 2018-05-07 | 2018-11-13 | 湖北大学 | LSCF/Na2CO3Nanocomposite is the preparation method of fuel cell ion transport layer |
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| US20090011307A1 (en) * | 2007-07-04 | 2009-01-08 | Korea Institute Of Science And Technology | Electrode-Electrolyte Composite Powders For a Fuel Cell And Method For The Preparation Thereof |
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| CN111584911A (en) * | 2020-05-11 | 2020-08-25 | 合肥学院 | Fe3O4-BCFN intermediate temperature composite solid electrolyte and preparation method thereof |
| CN111584911B (en) * | 2020-05-11 | 2022-11-01 | 合肥学院 | Fe3O4-BCFN intermediate temperature composite solid electrolyte and preparation method thereof |
| CN114068958A (en) * | 2021-11-16 | 2022-02-18 | 东南大学 | Method for preparing carbon nano tube by catalytic pyrolysis of waste plastics and applying carbon nano tube to low-temperature fuel cell |
| CN114068958B (en) * | 2021-11-16 | 2023-12-08 | 东南大学 | Method for preparing carbon nano tube by catalytic pyrolysis of waste plastics and applying carbon nano tube to low-temperature fuel cell |
| CN117410534A (en) * | 2023-11-08 | 2024-01-16 | 广东海洋大学 | Solid oxide fuel cell with symmetrical electrodes and preparation method thereof |
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